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单链DNA吸附在多壁碳纳米管上的实验证据

Experimental Evidence of Single-Stranded DNA Adsorption on Multiwalled Carbon Nanotubes.

作者信息

Tardani Franco, Sarti Stefano, Sennato Simona, Leo Manuela, Filetici Patrizia, Casciardi Stefano, Schiavi Pier Giorgio, Bordi Federico

机构信息

Istituto dei Sistemi Complessi (ISC) - CNR, UOS Roma Sapienza, Piazzale A. Moro 2, 00185 Roma, Italy.

Dipartimento di Medicina, Epidemiologi, Igiene del Lavoro e Ambientale, Istituto Nazionale per l'Assicurazione contro gli Infortuni sul Lavoro, Via Fontana Candida 1, 00078 Monte Porzio Catone RM, Italy.

出版信息

J Phys Chem B. 2020 Mar 26;124(12):2514-2525. doi: 10.1021/acs.jpcb.0c00882. Epub 2020 Mar 16.

Abstract

Noncovalent DNA functionalization is one of the most used routes for the easy dispersion of carbon nanotubes (CNTs) yielding DNA-CNTs complexes with promising applications. Definition of the structure of adsorbed DNA is crucial, but the organization of polymer at the carbon interface is far from being understood. In comparison to single-walled nanotubes, not much effort has been devoted to assessing the structure of the adsorbed DNA on multiwalled carbon nanotubes (MWCNTs), where their metallic nature, large size, and polydispersity represent serious obstacles for both experimental and theoretical studies. As a contribution to fill this lack in these aspects, we investigated DNA-MWCNT complexes by dielectric spectroscopy (DS) which is sensitive to even small changes in the charge distribution at charged interfaces and was largely employed in studying the electric and conformational properties of polyelectrolytes, such as DNA, in aqueous solutions and at interfaces. The dielectric relaxation in the MHz range is the signature of DNA adsorption on CNTs and sheds light on its conformational properties. A detailed analysis of the conductivity of the DNA-MWCNT suspensions unequivocally proves that DNA is adsorbed in a single-stranded conformation while excess DNA reassociates without interfering with the stability of the complexes.

摘要

非共价DNA功能化是实现碳纳米管(CNT)轻松分散的最常用途径之一,可生成具有广阔应用前景的DNA-CNT复合物。明确吸附DNA的结构至关重要,但聚合物在碳界面的组织情况仍远未明晰。与单壁纳米管相比,在评估多壁碳纳米管(MWCNT)上吸附DNA的结构方面投入的精力较少,MWCNT的金属性质、大尺寸和多分散性对实验和理论研究而言都是严重障碍。为弥补这些方面的不足,我们通过介电谱(DS)研究了DNA-MWCNT复合物,DS对带电界面电荷分布的微小变化很敏感,在研究诸如DNA等聚电解质在水溶液和界面处的电学及构象性质方面有广泛应用。兆赫兹范围内的介电弛豫是DNA吸附在CNT上的特征,有助于揭示其构象性质。对DNA-MWCNT悬浮液电导率的详细分析明确证明,DNA以单链构象吸附,而过量DNA重新结合且不影响复合物的稳定性。

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